Electrochemical CO2 Reduction with Atomic Iron‐Dispersed on Nitrogen‐Doped Graphene. Issue 19 (25th March 2018)

• Record Type: Journal Article
• Authors: Zhang, Chenhao; Yang, Shize; Wu, Jingjie; Liu, Mingjie; Yazdi, Sadegh; Ren, Muqing; Sha, Junwei; Zhong, Jun; Nie, Kaiqi; Jalilov, Almaz S.; Li, Zhenyuan; Li, Huaming; Yakobson, Boris I.; Wu, Qin; Ringe, Emilie; Xu, Hui; Ajayan, Pulickel M.; Tour, James M.
• Is Part Of: Advanced energy materials. Volume 8:Issue 19(2018)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2018-03-25
• Subjects: atomic iron -- CO2 reduction reaction -- electrocatalysts -- nitrogen‐doped graphene; Energy harvesting -- Materials -- Periodicals; Energy conversion -- Materials -- Periodicals; Energy storage -- Materials -- Periodicals; Photovoltaics -- Periodicals; Fuel cells -- Periodicals; Thermoelectric materials -- Periodicals; 621.31
• DOI: 10.1002/aenm.201703487
• Languages: English
• ISSNs: 1614-6832

Abstract

Abstract: Electrochemical reduction of CO2 provides an opportunity to reach a carbon‐neutral energy recycling regime, in which CO2 emissions from fuel use are collected and converted back to fuels. The reduction of CO2 to CO is the first step toward the synthesis of more complex carbon‐based fuels and chemicals. Therefore, understanding this step is crucial for the development of high‐performance electrocatalyst for CO2 conversion to higher order products such as hydrocarbons. Here, atomic iron dispersed on nitrogen‐doped graphene (Fe/NG) is synthesized as an efficient electrocatalyst for CO2 reduction to CO. Fe/NG has a low reduction overpotential with high Faradic efficiency up to 80%. The existence of nitrogen‐confined atomic Fe moieties on the nitrogen‐doped graphene layer is confirmed by aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy and X‐ray absorption fine structure analysis. The Fe/NG catalysts provide an ideal platform for comparative studies of the effect of the catalytic center on the electrocatalytic performance. The CO2 reduction reaction mechanism on atomic Fe surrounded by four N atoms (Fe–N4 ) embedded in nitrogen‐doped graphene is further investigated through density functional theory calculations, revealing a possible promotional effect of nitrogen doping on graphene. Abstract : Atomic iron‐dispersed on nitrogen‐doped graphene (Fe/NG) is synthesized here as an efficient electrocatalyst for CO2 reduction to CO. Fe/NG has a low reduction overpotential with high Faradic efficiency up to 80%. The Fe/NG catalysts provide an ideal platform for comparative studies of the effect of catalytic center on the electrocatalytic performance.